Maximizing orientation of a three-state molecule in a cavity with analytically designed pulses

TL;DR

This paper develops analytical control schemes to maximize the orientation of a three-state molecule in a cavity, achieving the same maximum orientation as free molecules through precise pulse design.

Contribution

It introduces two novel control schemes and pulse-area theorems for maximizing molecular orientation in cavity polaritons, extending control techniques to three-state molecules.

Findings

Maximum orientation of 0.7746 achieved theoretically

Control schemes validated through numerical simulations

Sensitivity analysis of control field parameters conducted

Abstract

We theoretically explore the precise control of a molecular polariton by strongly coupling the lowest three rotational states of a single molecule with a single-mode cavity. We examine two distinct cavity resonance configurations: a fundamental frequency cavity ($\omega_c = 2B$ with the rotational constant $B$) resonating with the lowest two rotational states, and a second harmonic cavity ($\omega_c = 4B$) coupling with the first and second excited rotational states. We propose two control schemes based on the two polariton configurations and derive the corresponding pulse-area theorems to achieve a theoretical maximum orientation of 0.7746, identical to the molecule in the absence of the cavity. The control schemes are analyzed in Carbonyl Sulfide (OCS) molecules in their ground rotational state. Our numerical simulation results demonstrate the theoretical control schemes and analyze the sensitivity of the molecular polariton orientation degree to the control field bandwidth and phases. This work provides a valuable reference for achieving maximum field-free orientation of ultracold three-state molecules in a cavity using analytically designed pulses.